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Physical review. B, Condensed matter

Two-photon excitation of Ho3+ in the Ca F2 , Sr F2 , and Cd F2 lattices

D. Narayana Rao, Jagdish Prasad, Paras N. Prasad

Published Jul 1, 1983• 22 citations
Publisher

Abstract

The observation of two-photon absorption by a very efficient up-converted emission is reported for ${\mathrm{Ho}}^{3+}$ in Ca${\mathrm{F}}_{2}$, Sr${\mathrm{F}}_{2}$, and Cd${\mathrm{F}}_{2}$ with both cw- and pulse-laser excitations. The two-photon excitation spectra are found to be highly structured and consist of two bands: The band $A$ is excited by the dye-laser photons of frequencies 15 400-15 700 ${\mathrm{cm}}^{\ensuremath{-}1}$: The band $B$ is excited by the dye-laser photons of frequencies 15 800-16 400 ${\mathrm{cm}}^{\ensuremath{-}1}$. No one-photon absorption is observed for ${\mathrm{Ho}}^{3+}$ in the above lattices at twice these frequencies. Studies of concentration dependence, temperature dependence, and dependence on the pulse repetition rate are used for the assignment of the band. The investigation shows that the two bands $A$ and $B$ arise from two different modes of two-photon excitation. The band $A$ is assigned to arise from a sequential (stepwise) two-photon excitation $^{5}I_{8}\ensuremath{\rightarrow}^{5}F_{5}\ensuremath{\rightarrow}^{5}D_{2}$. The band $B$ is assigned to arise from the direct two-photon absorption $^{5}I_{8}\ensuremath{\rightarrow}^{3}L_{8}$. Our results are in agreement with the prediction of the Judd-Ofelt theory of lanthanide transition intensities.

DOI
10.1103/physrevb.28.20

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The observation of two-photon absorption by a very efficient up-converted emission is reported for Ho3+{\mathrm{Ho}}^{3+}Ho3+ in CaF2{\mathrm{F}}_{2}F2​, SrF2{\mathrm{F}}_{2}F2​, and CdF2{\mathrm{F}}_{2}F2​ with both cw- and pulse-laser excitations. The two-photon excitation spectra are found to be highly structured and consist of two bands: The band AAA is excited by the dye-laser photons of frequencies 15 400-15 700 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1: The band BBB is excited by the dye-laser photons of frequencies 15 800-16 400 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1. No one-photon absorption is observed for Ho3+{\mathrm{Ho}}^{3+}Ho3+ in the above lattices at twice these frequencies. Studies of concentration dependence, temperature dependence, and dependence on the pulse repetition rate are used for the assignment of the band. The investigation shows that the two bands AAA and BBB arise from two different modes of two-photon excitation. The band AAA is assigned to arise from a sequential (stepwise) two-photon excitation 5I8\ensuremath→5F5\ensuremath→5D2^{5}I_{8}\ensuremath{\rightarrow}^{5}F_{5}\ensuremath{\rightarrow}^{5}D_{2}5I8​\ensuremath→5F5​\ensuremath→5D2​. The band BBB is assigned to arise from the direct two-photon absorption 5I8\ensuremath→3L8^{5}I_{8}\ensuremath{\rightarrow}^{3}L_{8}5I8​\ensuremath→3L8​. Our results are in agreement with the prediction of the Judd-Ofelt theory of lanthanide transition intensities.
Abstract Theoretical and experimental investigations are made of two‐photon absorption spectra of trivalent rare‐earth ions in crystals. Effective cross‐sections, selection rules, and relative intensities of the components are found. The most intensive two‐photon transitions are established. Two‐photon excitation spectra of luminescence of Er3+ and Ho3+ ions in CaF2 are obtained and effective excitation cross‐sections are measured using a tunable dye laser (715 to 850 nm). It is shown that the spectra have a peculiar structure which differs considerably from that of the one‐photon absorption spectra. The experimental results agree with theory. It is established that one of the levels in Ho3+ is the level 5G6 rather than 3K7 usually assumed.
With the use of laser-selective excitation, an extensive set of energy levels has been established for the principal Ho3+{\mathrm{Ho}}^{3+}Ho3+ dimer center in CsCdBr3{\mathrm{CsCdBr}}_{3}CsCdBr3​:Ho3+{\mathrm{Ho}}^{3+}Ho3+ crystals. The observed splittings of around 2 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ of the transitions to or from energy levels assigned as having ${\ensuremath{\gamma}}_{3}$ symmetry under C3v{\mathit{C}}_{3\mathit{v}}C3v​ symmetry is indicative of deviations of the Ho3+{\mathrm{Ho}}^{3+}Ho3+ ion-site symmetry from exact C3v{\mathrm{C}}_{3\mathit{v}}C3v​ symmetry. As for the previously studied Er3+{\mathrm{Er}}^{3+}Er3+ pair center in CsCdBr3{\mathrm{CsCdBr}}_{3}CsCdBr3​, the Ho3+{\mathrm{Ho}}^{3+}Ho3+ pair center exhibits strong upconversion fluorescence with up to one-third the intensity of the direct fluorescence under cw laser excitation of the 5^{5}5I8{\mathit{I}}_{8}I8​${\ensuremath{\rightarrow}}^{5}$S2{\mathit{S}}_{2}S2​ transition in the green and up to one-fifteenth the intensity for comparable cw laser excitation of the 5^{5}5I8{\mathit{I}}_{8}I8​${\ensuremath{\rightarrow}}^{5}$F5{\mathit{F}}_{5}F5​ transition in the red. Additional small splittings of up to 0.5 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ appear for the sharper transitions and are attributed to the ion-pair interaction. Energy levels are also reported for three varieties of minority centers with one of these centers being present in both 0.3% and 0.1% Ho3+{\mathrm{Ho}}^{3+}Ho3+ crystals, another in 0.01% Ho3+{\mathrm{Ho}}^{3+}Ho3+ crystals and the third in Na+{\mathrm{Na}}^{+}Na+ codoped crystals. Crystal-field analyses are reported for the principal dimer center and two of the minority centers. Fluorescence lifetimes were determined for several transitions of the dimer center and used to infer energy-transfer rates. Preliminary high-resolution results are reported for the excitation profiles of the two lowest-energy 5^{5}5I8{\mathit{I}}_{8}I8​${\ensuremath{\rightarrow}}^{5}$F5{\mathit{F}}_{5}F5​ transitions that show complex hyperfine patterns.
The possibility of observing two-photon processes using the intense beam of the ruby optical maser is considered theoretically for two general types of experiment. The essential approximation in the theory is the hypothesis that excited states exist which connect both the initial and final states by electric dipole transitions having a total oscillator strength $f\ensuremath{\sim}1$. Simple formulas are obtained for the two-photon absorption which do not depend on the details of the electronic structure. Recent experiments on the CaF2{\mathrm{F}}_{2}F2​: Eu++{\mathrm{Eu}}^{++}Eu++ system are in quantitative agreement with the predictions of the theory.
The polarised two-photon (IR) and one-photon (visible) luminescence excitation spectra of Nd 3+ nanoclusters in CaF 2 and SrF 2 crystals are measured at 10 K using a :LiF colour centre laser tunable in spectral ranges 1090 — 1230 nm and 545 — 615 nm with an emission linewidth of ~0.02 — 0.03 cm -1 , an average output power of ~55 mW, and a pulse repetition rate of 10 Hz. The two-photon excitation spectra at the 4 I 9/2 → 4 G 5/2 transition reveal the structure, which is absent upon one-photon excitation, which can be explained by different selection rules for some Stark — Stark transitions upon one- and two-photon absorption.
One-color two-photon excitation spectra of the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​ and 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​ transitions of Sm2+{\mathrm{Sm}}^{2+}Sm2+ in SrF2{\mathrm{SrF}}_{2}SrF2​ have been measured at low temperature and their dependences upon photon polarization analyzed. Linewidths on the order of 0.2, 0.6, and 1.0 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ are obtained for the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​(A1g{\mathit{A}}_{1\mathit{g}}A1g​), 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​(Eg{\mathit{E}}_{\mathit{g}}Eg​), and 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​(T2g{\mathit{T}}_{2\mathit{g}}T2g​) Stark components observed at 15 K, respectively. The 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​(A1g{\mathit{A}}_{1\mathit{g}}A1g​) transition is observed to be isotropic within experimental error, while the Eg{\mathit{E}}_{\mathit{g}}Eg​ and T2g{\mathit{T}}_{2\mathit{g}}T2g​ components of the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D2{\mathit{D}}_{2}D2​ transition exhibit the anisotropic patterns expected in Oh{\mathrm{O}}_{\mathit{h}}Oh​ symmetry. Calculations of two-photon transition intensities are conducted within the framework of the phenomenological model previously used for Sm2+{\mathrm{Sm}}^{2+}Sm2+ in MClF (M=Ba,Sr) and Eu3+{\mathrm{Eu}}^{3+}Eu3+ in LuPO4{\mathrm{LuPO}}_{4}LuPO4​, where the rare-earth ion occupies sites of C4v{\mathit{C}}_{4\mathit{v}}C4v​ and D2d{\mathit{D}}_{2\mathit{d}}D2d​ symmetries, respectively. The present results are compared and contrasted with those obtained in these previous cases.
The theory of one- and two-photon transitions between a given pair of impurity levels of the same parity is developed. As is well known, lattice vibrations assist the otherwise forbidden one-photon transition, increasing its intensity with temperature. The two-photon transition rate is shown to have a complementary decrease with increasing temperature. A measurement of both temperature dependences determines the effective frequency and coupling constant for the interaction. The formalism is applied to predicting the two-photon transition rate for the $4{d}^{10}\ensuremath{-}4{d}^{9}5s$ transition of the silver ion in NaCl:Ag. For an experiment using a ruby laser and an ultraviolet beam the maximum absorption coefficient predicted for the ultraviolet beam is $3.2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}48}\mathrm{FN}$ ${\mathrm{cm}}^{\ensuremath{-}1}$ at low temperatures, where FFF is the flux (photons/cm2{\mathrm{cm}}^{2}cm2 sec) of the laser and NNN is the Ag+{\mathrm{Ag}}^{+}Ag+ concentration. This should be within reach of present experimental techniques.